Статья

Hydrogen radical-boosted electrocatalytic CO2 reduction using Ni-partnered heteroatomic pairs

Zhibo YaoState Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing, PR ChinaHao ChengDepartment of Applied Physics, The Hong Kong Polytechnic University, Hung Hom, Hong Kong SAR, PR ChinaYifei XuCollege of Chemistry and Molecular Engineering, Peking University, Beijing, PR ChinaXinyu ZhanState Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing, PR ChinaSong HongState Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing, PR ChinaXinyi TanSchool of Materials Science and Engineering, Beijing Institute of Technology, Beijing Key Laboratory of Environmental Science and Engineering, Beijing, PR China. [email protected]Tai‐Sing WuNational Synchrotron Radiation Research Center, Hsinchu, TaiwanPei XiongDepartment of Applied Physics, The Hong Kong Polytechnic University, Hong Kong, PR ChinaY. L. SooDepartment of Physics, National Tsing Hua University, Hsinchu, TaiwanMolly Meng‐Jung LiDepartment of Applied Physics, The Hong Kong Polytechnic University, Hong Kong, PR ChinaLeiduan HaoState Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing, PR ChinaLiang XuState Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing, PR ChinaAlex W. RobertsonDepartment of Physics, University of Warwick, Coventry, UKBingjun XuCollege of Chemistry and Molecular Engineering, Peking University, Beijing, PR ChinaMing YangDepartment of Applied Physics, The Hong Kong Polytechnic University, Hung Hom, Hong Kong SAR, PR China. [email protected]Zhenyu SunState Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing, PR China. [email protected]

2024en

ABI

Аннотация

The electrocatalytic reduction of CO2 to CO is slowed by the energy cost of the hydrogenation step that yields adsorbed *COOH intermediate. Here, we report a hydrogen radical (H•)-transfer mechanism that aids this hydrogenation step, enabled by constructing Ni-partnered hetero-diatomic pairs, and thereby greatly enhancing CO2-to-CO conversion kinetics. The partner metal to the Ni (denoted as M) catalyzes the Volmer step of the water/proton reduction to generate adsorbed *H, turning to H•, which reduces CO2 to carboxyl radicals (•COOH). The Ni partner then subsequently adsorbs the •COOH in an exothermic reaction, negating the usual high energy-penalty for the electrochemical hydrogenation of CO2. Tuning the H adsorption strength of the M site (with Cd, Pt, or Pd) allows for the optimization of H• formation, culminating in a markedly improved CO2 reduction rate toward CO production, offering 97.1% faradaic efficiency (FE) in aqueous electrolyte and up to 100.0% FE in an ionic liquid solution. Commercially viable catalytic CO2 electroreduction to CO would enable many green technologies, yet it is impeded by the initial hydrogenation step of CO2. Here, the authors report Ni-Cd dual atom catalysts with complementary properties of favorable adsorption of CO2 and H to overcome this barrier.

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Идентификаторы

DOI: 10.1038/s41467-024-53529-2

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Цитирований: 2Использованных источников: 0

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